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US7521026B2 - Field-enhanced electrodes for additive-injection non-thermal plasma (NTP) processor - Google Patents

Field-enhanced electrodes for additive-injection non-thermal plasma (NTP) processor Download PDF

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Publication number
US7521026B2
US7521026B2 US11/017,392 US1739204A US7521026B2 US 7521026 B2 US7521026 B2 US 7521026B2 US 1739204 A US1739204 A US 1739204A US 7521026 B2 US7521026 B2 US 7521026B2
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electrode
field
high voltage
package
dielectric material
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Expired - Fee Related, expires
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US20050133927A1 (en
Inventor
Louis A. Rosocha
Vincent Ferreri
Yongho Kim
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Los Alamos National Security LLC
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Los Alamos National Security LLC
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Priority claimed from US10/395,046 external-priority patent/US7063819B2/en
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Assigned to REGENTS OF THE UNIVERSITY OF CALIFORNIA, THE reassignment REGENTS OF THE UNIVERSITY OF CALIFORNIA, THE ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: FERRERI, VINCENT, KIM, YONGHO, ROSOCHA, LOUIS A.
Publication of US20050133927A1 publication Critical patent/US20050133927A1/en
Assigned to ENERGY, U.S. DEPARTMENT OF reassignment ENERGY, U.S. DEPARTMENT OF CONFIRMATORY LICENSE (SEE DOCUMENT FOR DETAILS). Assignors: REGENTS OF THE UNIVERSITY OF CALIFORNIA, THE
Priority to PCT/US2005/040999 priority patent/WO2007035182A2/fr
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    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
    • H05H1/00—Generating plasma; Handling plasma
    • H05H1/24—Generating plasma
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
    • B01D53/323—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00 by electrostatic effects or by high-voltage electric fields
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J19/087—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J19/088—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J37/00—Discharge tubes with provision for introducing objects or material to be exposed to the discharge, e.g. for the purpose of examination or processing thereof
    • H01J37/32—Gas-filled discharge tubes
    • H01J37/32009—Arrangements for generation of plasma specially adapted for examination or treatment of objects, e.g. plasma sources
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J37/00—Discharge tubes with provision for introducing objects or material to be exposed to the discharge, e.g. for the purpose of examination or processing thereof
    • H01J37/32—Gas-filled discharge tubes
    • H01J37/32009—Arrangements for generation of plasma specially adapted for examination or treatment of objects, e.g. plasma sources
    • H01J37/32348—Dielectric barrier discharge
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
    • H05H1/00—Generating plasma; Handling plasma
    • H05H1/24—Generating plasma
    • H05H1/2406—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes
    • H05H1/2443—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes the plasma fluid flowing through a dielectric tube
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2259/00—Type of treatment
    • B01D2259/80—Employing electric, magnetic, electromagnetic or wave energy, or particle radiation
    • B01D2259/818—Employing electrical discharges or the generation of a plasma
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0809—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes employing two or more electrodes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0824—Details relating to the shape of the electrodes
    • B01J2219/0826—Details relating to the shape of the electrodes essentially linear
    • B01J2219/083—Details relating to the shape of the electrodes essentially linear cylindrical
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0824—Details relating to the shape of the electrodes
    • B01J2219/0835—Details relating to the shape of the electrodes substantially flat
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0837—Details relating to the material of the electrodes
    • B01J2219/0841—Metal
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0869—Feeding or evacuating the reactor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0873—Materials to be treated
    • B01J2219/0875—Gas
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0894—Processes carried out in the presence of a plasma
    • B01J2219/0896—Cold plasma

Definitions

  • the present invention relates generally to non-thermal plasma processors, and, more particularly, to electrodes used in non-thermal plasma processors.
  • the present invention has recognized these prior art drawbacks, and employs electrical discharges/non-thermal plasmas in a gaseous medium to destroy air pollutants or undesirable chemicals/chemical or biological agents; process chemicals, or synthesize chemical compounds.
  • non-thermal plasmas the electrons are “hot”, while the ions and neutral species are “cold” which results in little waste enthalpy being deposited in a process gas stream. This is in contrast to thermal plasmas, where the electron, ion, and neutral-species energies are in thermal equilibrium (or “hot”) and considerable waste heat is deposited in the process gas.
  • the present invention improves formation of active species formed from the injection of additive gases/chemical compounds into a process gas stream to increase the efficiency and/or selectivity of the plasma processing by providing a shaped injection electrode that enhances and/or tailors the electric field near the additive-gas injection holes/ports.
  • the present invention includes a field enhanced electrode package for use in a non-thermal plasma processor.
  • the field enhanced electrode package includes a high voltage electrode and a field-enhancing electrode with a dielectric material layer disposed in-between the high voltage electrode and the field-enhancing electrode.
  • the field-enhancing electrode features at least one raised section that includes at least one injection hole that allows plasma discharge streamers to occur primarily within an injected additive gas.
  • FIG. 1 pictorially shows one embodiment of a shape for the present invention showing a coaxial-cylinder configuration of the additive-gas injection, field-enhanced electrode concept, using a silent discharge plasma (dielectric-barrier discharge) non-thermal plasma reactor.
  • a silent discharge plasma dielectric-barrier discharge
  • FIG. 2 pictorially shows another embodiment of a shape for the present invention of a field-enhanced injection electrode using a hollow, screw-thread electrode.
  • FIG. 3 pictorially shows another embodiment of the present invention including an additional one or more helical hollow tube electrodes.
  • the subject technology uses a silent-discharge/dielectric-barrier non-thermal plasma (NTP) processor to generate highly reactive chemical species (such as free radicals).
  • NTP non-thermal plasma
  • reactive species (0-atoms, OH-radicals, N-radicals, excited N 2 and O 2 molecules, HO 2 -radicals, NH-radicals, CH-radicals, etc.) readily decompose organic chemicals (e.g., VOCs), oxides of sulfur and nitrogen (S0 2 and NO x ), and odor agents (e.g., aldehydes, H 2 S, and many others), breaking their chemical bonds and producing non-hazardous or easily managed products.
  • These radicals can also play a key role in chemical synthesis, producing desirable products (e.g., creating higher-order hydrocarbon fuels from methane/natural gas).
  • the processor makes use of a dielectric-barrier discharge arrangement.
  • two conducting electrodes, high voltage electrode 24 and field enhancing electrode 26 are in proximity to one another, separated by gas modification passage 30 , where the discharge gap is defined by dimension H ranging from 1-10 mm.
  • High-voltage source 22 (alternating current, frequency in a typical range of 10 Hz-20 kHz) is applied to high voltage electrode 24 , creating electrical-discharge streamers in process gas 31 that flows through gas modification passage 30 .
  • the discharges are the source of the active non-thermal plasma.
  • Such an NTP unit is able to reduce the concentration of hazardous compound in off-gases to very low levels by free-radical “cold combustion” or to synthesize desirable chemical products using gaseous feedstocks. Because this invention provides for the injection of additive chemical compounds (e.g., ammonia, hydrocarbons, etc.) into the activated process gas stream, additional reactive species are created.
  • additive chemical compounds e.g., ammonia, hydrocarbons, etc.
  • the improvement provided by the present invention resides in the shape of field enhancing electrode 26 to include raised sections 33 surrounding additive-gas injection holes 34 that reduce the distance between high voltage electrode 24 and field enhancing electrode 26 , and, thus reduce discharge gap H by distance h (where h ⁇ H).
  • Raised sections 33 enhance the electric field, by factors ranging from 2 to 100, in close proximity to injection holes 34 by virtue of the geometrical configuration (e.g sharpness), allowing plasma/active-species formation in additive gas 37 . This results in more plasma energy being channeled into the creation of active species in additive-gas 37 streams and less non-productive energy being deposited into electrical discharge streamers in process gas 31 stream.
  • SDP/DBD processor 10 can be used to generate highly reactive chemical species, such as free radicals, that break chemical bonds, as described above.
  • Gases that may be used as process gases 31 include, but are not limited to, stack/flue/exhaust gases containing HAPs:(hazardous air pollutants), volatile organic compounds (VOCs), hydrocarbons, chlorocarbons, chloro-fluorocarbons, fluorocarbons, oxides of nitrogen and sulfur, hydrogen sulfide, various odors (e.g., aldehydes), chemical or biological warfare agents, or airborne pathogens; the defining characteristics of this group being toxicity, hazard, pathogenecity, or odor.
  • stack/flue/exhaust gases containing HAPs containing HAPs:(hazardous air pollutants), volatile organic compounds (VOCs), hydrocarbons, chlorocarbons, chloro-fluorocarbons, fluorocarbons, oxides of nitrogen and sulfur, hydrogen sulfide, various odors (e.g., aldehydes), chemical or biological warfare agents, or airborne pathogens; the defining characteristics of this group being toxicity
  • Gases that may be used as additive gases 37 include, but are not limited to, methane, ethane, propane, butane, propene, and other organic hydrocarbons, and ammonia, helium, argon, and nitrogen; the defining characteristics of this group being the ability to form free-radical, excited-state, or ionized active species in a plasma.
  • Conductive electrodes 24 , 26 Materials that may be used for conducting electrodes 24 , 26 include aluminum, copper, brass, stainless steel, inconel, titanium, tungsten, and alloyed metals.
  • the preferred materials for conducting electrodes 24 , 26 are stainless steel, or any other corrosion-resistant metal, when acid-gases are processed or produced.
  • Dielectric materials that may be used as a coating include glass, fused silica (quartz), ceramics, porcelain, diamond, or diamond-like carbon; the preferred materials being fused silica and ceramics because of the favorable dielectric constants, mechanical/chemical durability, and relatively low dielectric power loss.
  • the SDP/DBD processor high-voltage source 22 is operated in a range of 1 Hz-50 kHz in either continuous, intermittent duty, or pulse trains. If pulse trains are employed, they exhibit pulse durations from 5 nanoseconds to 100's of microseconds, with corresponding pulse repetition frequency ranging from 1 Hz to 50 kHz, more preferably in a range of 50 Hz to 20 kHz.
  • the voltage supplied to the electrode 24 is dependent on the process gas composition and pressure, and discharge gap H. Typically, this would be 5 to 50 kV peak voltage for near-atmospheric pressure air streams with a few millimeter electrode gap spacing.
  • raised sections 33 may be formed in any geometrical configuration (conical, square, triangular, hemispherical, etc.), where angle ⁇ is greater than 0 degrees and less than or equal to 90 degrees.
  • the geometric configuration shown here is conical.
  • FIG. 2 another embodiment of the field-enhancing electrode takes the shape of a hollow threaded screw, where raised sections 33 are in the form of threads with injection holes 34 placed at the top of the thread.
  • one or more tubes T n , T n+1 which define injection holes 38 , are wrapped in a helix configuration around injection electrode 26 , within gas modification passage 30 .
  • One or more tubes T n , T n+1 are adjacent to, or in intimate contact with, electrode 24 .
  • An additive gas flows through one or more tubes T n , T n+1 , exiting into gas modification passage 30 , creating an environment for pre-ionization of gases within passage 30 . This configuration allows for an enhanced, uniform, bulk discharge of the NTP during operation.
  • a separate power supply HV n energizes pre-ionization electrode T n to create ions for seeding the main electrical-discharge plasma in gas modification passage 30 .
  • This separate power supply can be connected between electrode T n and field enhancing electrode 26 , or between electrode T n and outer electrode 24 .
  • differing high voltage supplies HV n+1 can be connected to additional electrodes T n+1 , creating any number of differing voltage potentials that provide for continued enhancement of a uniform bulk discharge of the NTP.
  • electrode T n , T n+1 surfaces create discharges that lead to creating additional active species (including UV photons) for processing the gas in passage 30 .
  • Material composition of electrodes T n , T n+1 include, but are not limited to: aluminum, copper, brass, stainless steel, inconel, titanium, tungsten, and alloyed metals, and in a preferred embodiment comprise stainless steel or any other corrosion-resistant metal, when acid-gases are processed or produced.
  • Voltages HV n , HV n+1 range from 5 kV to 100 kV, more preferably from 5 kV to 50 kV due to the ease of one skilled in the art to design and construct arc-free plasma chemical reactors and electrical feedthroughs/connectors in this voltage range.
  • the addition of a dielectric coating to electrode 26 increases the efficiency of coupling electrical energy into the injected gas by as the dielectric coating allows for proper matching of he power supply impedance to the plasma/electrical discharge impedance.
  • the dielectric layer also prevents the formation of thermal arcs in the process gas and/or the injection gas.

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  • Chemical & Material Sciences (AREA)
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US11/017,392 2003-03-21 2004-12-20 Field-enhanced electrodes for additive-injection non-thermal plasma (NTP) processor Expired - Fee Related US7521026B2 (en)

Priority Applications (2)

Application Number Priority Date Filing Date Title
US11/017,392 US7521026B2 (en) 2003-03-21 2004-12-20 Field-enhanced electrodes for additive-injection non-thermal plasma (NTP) processor
PCT/US2005/040999 WO2007035182A2 (fr) 2004-12-20 2005-11-14 Électrodes à champ amplifié de processeur au plasma non thermique à injection d’additif

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US10/395,046 US7063819B2 (en) 2003-03-21 2003-03-21 Nonthermal plasma processor utilizing additive-gas injection and/or gas extraction
US11/017,392 US7521026B2 (en) 2003-03-21 2004-12-20 Field-enhanced electrodes for additive-injection non-thermal plasma (NTP) processor

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US10/395,046 Continuation-In-Part US7063819B2 (en) 2003-03-21 2003-03-21 Nonthermal plasma processor utilizing additive-gas injection and/or gas extraction

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CN111298608B (zh) * 2020-03-03 2021-03-23 云南大学 一种用于等离子体降解VOCs装置的自清洁防火系统
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US6365112B1 (en) * 2000-08-17 2002-04-02 Sergei Babko-Malyi Distribution of corona discharge activated reagent fluid injected into electrostatic precipitators

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US20110075313A1 (en) * 2009-09-30 2011-03-31 Keith Comendant Plasma arrestor insert
US8503151B2 (en) * 2009-09-30 2013-08-06 Lam Research Corporation Plasma arrestor insert

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